Abstract
Single-atom catalysts (SACs) are highly enviable to exploit the utmost utilization of metallic catalysts; their efficiency by utilizing nearly all atoms to often exhibit high catalytic performances. To architect the isolated single atom on an ideal solid support with strong coordination has remained a crucial trial. Herein, graphene functionalized with nitrile groups (cyanographene) as an ideal support to immobilize isolated copper atoms G(CN)-Cu with strong coordination is reported. The precisely designed mixed-valence single atom copper (G(CN)-Cu) catalysts deliver exceptional conversions for electrochemical methanol oxidation (MOR) and CO2 reduction (CO2RR) targeting a "closed carbon cycle." An onset of MOR and CO2RR are obtained to be approximate to 0.4 V and approximate to-0.7 versus Ag/AgCl, respectively, with single active sites located in an unsaturated coordination environment, it being the most active Cu sites for both studied reactions. Moreover, G(CN)-Cu exhibited significantly lower resistivity and higher current density toward MOR and CO2RR than observed for reference catalysts.